Coordination Confined Silver‐Organic Framework for High Performance Electrochemical Deionization.

Silver (Ag) is deemed a promising anode material for capacitive deionization (CDI) due to its high theoretical capacity and efficient selectivity to Cl−. However, the strong volume change during the conversion reaction significantly undermines the cycling performance of the Ag electrode. Additionally, achieving well‐dispersed Ag in the active matrix is challenging, as Ag electrodes prepared by conventional thermal reduction tend to agglomerate. Herein, the organic linker confinement strategy is proposed, applying metal–organic framework (MOF) chemistry between Ag nodes and organic ligands to construct Ag‐based MOF. The uniform dispersion of Ag at the molecular level, confined in the organic matrix, efficiently enhances the utilization of active sites, and strengthens the interfacial stability of Ag. Consequently, the Ag‐MOF for the CDI anode exhibits an excellent Cl− removal capacity of 121.52 mg g−1 at 20 mA g−1 in 500 mg L−1 NaCl solution, and a high Ag utilization rate of 60.54%. After 100 cycles, a capacity retention of 96.93% is achieved. Furthermore, the Cl− capture mechanism of Ag‐MOF is elucidated through density functional theory (DFT) calculations, ex situ XRD, ex situ Raman and XPS. This ingenious electrode design can offer valuable insights for the development of high‐performance conversion electrodes for CDI applications. [ABSTRACT FROM AUTHOR]